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Concurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide

Electrosynthesis of hydrogen peroxide via selective two-electron transfer oxygen reduction or water oxidation reactions offers a cleaner, cost-effective alternative to anthraquinone processes. However, it remains a challenge to achieve high Faradaic efficiencies at elevated current densities. Herein...

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Autores principales: Kim, Changmin, Park, Sung O, Kwak, Sang Kyu, Xia, Zhenhai, Kim, Guntae, Dai, Liming
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10509222/
https://www.ncbi.nlm.nih.gov/pubmed/37726271
http://dx.doi.org/10.1038/s41467-023-41397-1
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author Kim, Changmin
Park, Sung O
Kwak, Sang Kyu
Xia, Zhenhai
Kim, Guntae
Dai, Liming
author_facet Kim, Changmin
Park, Sung O
Kwak, Sang Kyu
Xia, Zhenhai
Kim, Guntae
Dai, Liming
author_sort Kim, Changmin
collection PubMed
description Electrosynthesis of hydrogen peroxide via selective two-electron transfer oxygen reduction or water oxidation reactions offers a cleaner, cost-effective alternative to anthraquinone processes. However, it remains a challenge to achieve high Faradaic efficiencies at elevated current densities. Herein, we report that oxygen-deficient Pr(1.0)Sr(1.0)Fe(0.75)Zn(0.25)O(4-δ) perovskite oxides rich of oxygen vacancies can favorably bind the reaction intermediates to facilitate selective and efficient two-electron transfer pathways. These oxides exhibited superior Faradic efficiencies (~99%) for oxygen reduction over a wide potential range (0.05 to 0.45 V versus reversible hydrogen electrode) and current densities surpassing 50 mA cm(−2) under high ionic strengths. We further found that the oxides perform a high selectivity (~80%) for two-electron transfer water oxidation reaction at a low overpotential (0.39 V). Lastly, we devised a membrane-free electrolyser employing bifunctional electrocatalysts, achieving a record-high Faradaic efficiency of 163.0% at 2.10 V and 50 mA cm(−2). This marks the first report of the concurrent oxygen reduction and water oxidation catalysed by efficient bifunctional oxides in a novel membrane-free electrolyser for scalable hydrogen peroxide electrosynthesis.
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spelling pubmed-105092222023-09-21 Concurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide Kim, Changmin Park, Sung O Kwak, Sang Kyu Xia, Zhenhai Kim, Guntae Dai, Liming Nat Commun Article Electrosynthesis of hydrogen peroxide via selective two-electron transfer oxygen reduction or water oxidation reactions offers a cleaner, cost-effective alternative to anthraquinone processes. However, it remains a challenge to achieve high Faradaic efficiencies at elevated current densities. Herein, we report that oxygen-deficient Pr(1.0)Sr(1.0)Fe(0.75)Zn(0.25)O(4-δ) perovskite oxides rich of oxygen vacancies can favorably bind the reaction intermediates to facilitate selective and efficient two-electron transfer pathways. These oxides exhibited superior Faradic efficiencies (~99%) for oxygen reduction over a wide potential range (0.05 to 0.45 V versus reversible hydrogen electrode) and current densities surpassing 50 mA cm(−2) under high ionic strengths. We further found that the oxides perform a high selectivity (~80%) for two-electron transfer water oxidation reaction at a low overpotential (0.39 V). Lastly, we devised a membrane-free electrolyser employing bifunctional electrocatalysts, achieving a record-high Faradaic efficiency of 163.0% at 2.10 V and 50 mA cm(−2). This marks the first report of the concurrent oxygen reduction and water oxidation catalysed by efficient bifunctional oxides in a novel membrane-free electrolyser for scalable hydrogen peroxide electrosynthesis. Nature Publishing Group UK 2023-09-19 /pmc/articles/PMC10509222/ /pubmed/37726271 http://dx.doi.org/10.1038/s41467-023-41397-1 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Kim, Changmin
Park, Sung O
Kwak, Sang Kyu
Xia, Zhenhai
Kim, Guntae
Dai, Liming
Concurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide
title Concurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide
title_full Concurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide
title_fullStr Concurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide
title_full_unstemmed Concurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide
title_short Concurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide
title_sort concurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10509222/
https://www.ncbi.nlm.nih.gov/pubmed/37726271
http://dx.doi.org/10.1038/s41467-023-41397-1
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